Dracocephalum moldavica L. (Moldavian dragonhead), an aromatic herb with useful medicinal properties, is widely cultivated in northwest Iran. Different bioactive constituents of essential oil from the plants have been suggested to contribute to the sedative, painkiller properties [1] and anti-helicobacter pylori activity of this plant [2]. Seven cultivated populations (landraces) of D. moldavica L. was studied in the present work. Inter-simple sequence repeat (ISSR) molecular markers and analysis of essential oils’ compositions were used to evaluate genetic polymorphisms, population structure, and phytochemical diversity among and within populations. The studied individuals in populations were distinguished, based on quantity and quality of essential oils and ISSR markers. Essential oil yields of the seven landraces studied, varied from 5.62 to 13.97 kg/hectare. Essential oil compounds were found to be extremely variable in the various individuals. Geranyl acetate (19.8-45.5%), Geranial (20.22-25.60%), and Neral (15.8-18.5%) were determined as the dominant compounds. A total of 94 bands were produced by 14 ISSR primers, among which 91.4% were found to be polymorphic. The degree of genetic similarity among individuals varied between 0.15 and 0.75, which is indicative of a high level of genetic diversity. Cluster analysis, population inference, and principal coordinates analysis (PCoA) based on ISSR molecular data confirmed the high level of variation, and divided samples into two main groups. In the first group, Moldavian Balm populations included Keshtiban (West Azerbaijan), Jahangir and Shiraz Valley (East Azerbaijan). Further the populations of the Keshtiban, Topragh Ghalee, Baghchajogh, Naghadeh (West Azerbaijan), Jahangir and Hokmabad (East Azerbaijan) were placed in the second group. Understanding the phytochemical diversity and genetic in the landraces of dragonhead can be beneficial in germplasm management and plant improvement, in the context of pharmaceutic